By conducting experimental analyses, including thermal pyrolysis, micro-/nano-CT, argon-ion polishing field emission scanning electron microscopy (FE-SEM), confocal laser scanning microscopy (CLSM), and two-dimensiona...By conducting experimental analyses, including thermal pyrolysis, micro-/nano-CT, argon-ion polishing field emission scanning electron microscopy (FE-SEM), confocal laser scanning microscopy (CLSM), and two-dimensional nuclear magnetic resonance (2D NMR), the Gulong shale oil in the Songliao Basin was investigated with respect to formation model, pore structure and accumulation mechanism. First, in the Gulong shale, there are a large number of pico-algae, nano-algae and dinoflagellates, which were formed in brackish water environment and constituted the hydrogen-rich oil source materials of shale. Second, most of the oil-generating materials of the Qingshankou Formation shale exist in the form of organo-clay complex. During organic matter thermal evolution, clay minerals had double effects of suppression and catalytic hydrogenation, which expanded shale oil window and increased light hydrocarbon yield. Third, the formation of storage space in the Gulong Shale was related to dissolution and hydrocarbon generation. With the diagenesis, micro-/nano-pores increased, pore diameter decreased and more bedding fractures appeared, which jointly gave rise to the unique reservoir with dual media (i.e. nano-scale pores and micro-scale bedding fractures) in the Gulong shale. Fourth, the micro-/nano-scale oil storage unit in the Gulong shale exhibits independent oil/gas occurrence phase, and shows that all-size pores contain oils, which occur in condensate state in micropores or in oil-gas two phase (or liquid) state in macropores/mesopores. The understanding about Gulong shale oil formation and accumulation mechanism has theoretical and practical significance for advancing continental shale oil exploration in China.展开更多
On the basis of sorting out current understanding of solid bitumen (SB) in shales and taking organic-rich shales in the first member of the Cretaceous Qingshankou Formation in the Songliao Basin as an example, the def...On the basis of sorting out current understanding of solid bitumen (SB) in shales and taking organic-rich shales in the first member of the Cretaceous Qingshankou Formation in the Songliao Basin as an example, the definition, classification, occurrence and evolution path of SB are systemtically studied, and the indicative significance of SB reflectance (Rob) on maturity and its influence on the development of reservoir space are discussed and summarized. The results show that the difference of primary maceral types is primarily responsible for the different evolution paths of SB. Most of the pre-oil bitumen is in-situ SB with only a small amount being of migrated SB, while most of the post-oil bitumen and pyrobitumen are migrated SB. From the immature to early oil maturity stage, bituminite, vitrinite, and inertinite can be distinguished from SB based on their optical characteristics under reflected light, and alginite can be differentiated from SB by their fluorescence characteristics. Under scanning electron microscope, in-situ SB and migrated SB can be effectively identified. Rob increases linearly with increasing vitrinite reflectance (Ro), as a result of a decrease of aliphatic structure and the enhancement of aromatization of SB. Within the oil window three types of secondary pores may develop in SB, including modified mineral pores, devolatilization cracks and bubble holes. At a high maturity stage spongy pores may develop in pyrobitumen. Scanning electron microscopy combined with in-situ SEM-Raman spectroscopy can further reveal the structral information of different types of SB, thus providing crucial data for understanding for understanding OM migration paths, dynamics, and distances at micro-scale.展开更多
In order to investigate the migration and accumulation efficiency of hydrocarbon natural gas in the Xujiaweizi fault depression, and to provide new evidence for the classification of its genesis, a source rock pyrolys...In order to investigate the migration and accumulation efficiency of hydrocarbon natural gas in the Xujiaweizi fault depression, and to provide new evidence for the classification of its genesis, a source rock pyrolysis experiment in a closed system was designed and carried out. Based on this, kinetic models for describing gas generation from organic matter and carbon isotope fractionation during this process were established, calibrated and then extrapolated to geologic conditions by combining the thermal history data of the Xushen-1 Well. The results indicate that the coal measures in the Xujiaweizi fault depression are typical "high-efficiency gas sources", the natural gas generated from them has a high migration and accumulation efficiency, and consequently a large-scale natural gas accumulation occurred in the area. The highly/over matured coal measures in the Xujiaweizi fault depression generate coaliferous gas with a high δ^13C1 value (〉 -20‰) at the late stage, making the carbon isotope composition of organic alkane gases abnormally heavy. In addition, the mixing and dissipation through the caprock of natural gas can result in the negative carbon isotope sequence (δ^13C1 〉δ^13C2 〉δ^13C3 〉δ^13C4) of organic alkane gases, and the dissipation can also lead to the abnormally heavy carbon isotope composition of organic alkane gases. As for the discovery of inorganic nonhydrocarbon gas reservoirs, it can only serve as an accessorial evidence rather than a direct evidence that the hydrocarbon gas is inorganic. As a result, it needs stronger evidence to classify the hydrocarbon natural gas in the Xujiaweizi fault depression as inorganic gas.展开更多
Taking tight oil in Gaotaizi and Fuyu oil layers of the Upper Cretaceous Qingshankou Formation in northern Songliao Basin as an example, based on analyses of nuclear magnetic resonance and high pressure mercury inject...Taking tight oil in Gaotaizi and Fuyu oil layers of the Upper Cretaceous Qingshankou Formation in northern Songliao Basin as an example, based on analyses of nuclear magnetic resonance and high pressure mercury injection, experiment methods of supercritical carbon dioxide displacement and extraction are firstly employed to quantify crude oil mobility in tight sand reservoirs with different lithologies and oil contents. The results show that, under the conditions of simulating the Cretaceous Qingshankou Formation in the northern Songliao Basin at a temperature of 76-89 °C and a pressure of 35-42 MPa, the lower limit of the porosity of the movable oil is4.4%, and the lower limit of the permeability is 0.015′10-3 mm2. The lower limit of the average pore throat radius is 21 nm. On this basis,a classification standard for three types of tight sand reservoirs is proposed. Type I reservoirs are characterized by the movable fluid saturation larger than 40%, the movable oil ratio(ratio of movable oil to total oil) greater than 30% and the starting pressure gradient in the range of 0.3-0.6 MPa/m; Type II reservoirs are characterized by the movable fluid saturation in the range of 10%–40%, the movable oil ratio in the range of 5%–30% and the starting pressure gradient in the range of 0.6–1.0 MPa/m; Type III reservoirs are characterized by the movable fluid saturation less than 10% in general, the movable oil ratio less than 5%, and the starting pressure gradient greater than1.0 MPa/m. The fluid mobility in tight sand reservoirs is mainly affected by diagenesis and sedimentary environment. Reservoirs with depth lower than 2000 m are dominated by type I reservoir, whereas those with greater depth are dominated by type I and II reservoirs.Reservoirs in inner delta-front facies are dominated by type I reservoir, whereas those in outer delta-front facies and shore-shallow lacustrine facies are dominated by type II and III reservoirs.展开更多
1 Introduction The technology breakthrough in the exploration of shale gas and tight oil has greatly extended the global fossil fuel resources (Jia et al., 2012; Zou et al., 2012; Qiu et al., 2013). Although shale o...1 Introduction The technology breakthrough in the exploration of shale gas and tight oil has greatly extended the global fossil fuel resources (Jia et al., 2012; Zou et al., 2012; Qiu et al., 2013). Although shale oil has been the global hot topic in the study of unconventional resources, there are varied definitions with respect to shale oil by different researchers.展开更多
Several oil shale beds, over 10 m thick, occur at the base of the first member of the Upper Cretaceous Qingshankou Formation (K2qn1) in the Songliao Basin. They act both as excellent source rocks for conventional oil ...Several oil shale beds, over 10 m thick, occur at the base of the first member of the Upper Cretaceous Qingshankou Formation (K2qn1) in the Songliao Basin. They act both as excellent source rocks for conventional oil and as potential oil deposit for shale oil production. Here we combine micropaleon-tology with organic geochemistry to investigate the paleo-depositional environment and organic source characteristics of the oil shales and black shales. Our results indicate that algal remains are dominant microfossils in K2qn1 oil shales, and their relatively high abundance suggests a major algal thriving event during the oil shale deposition. The presence of fresh water and brackish water species, Sentusidinium, Vesperopsis and Nyktericysta, and marine or brackish water deltaic and lagoonal species such as Kiokansium and Dinogymniopsis demonstrate that this paleo-continental lake was influenced by marine transgressions at the time of K2qn1 oil shale formation. The extremely low pristine/phytane ratios, relatively high abundance of gammacerane and 4-methyl steranes, and low δ 13C values of C14-C37 n-alkanes in the oil shale organic extracts indicate the deposition of oil shales in anoxic and highly stratified water columns and the significant contribution of lacustrine algae to sedimentary organic matter. High molecular-weight paraffinic hydrocarbons with unusually high abundance of nC43, nC45, and nC47 may be related to special algal species associated with marine transgression events. The giant water body of Songliao paleo-lake and the change in the organic and chemical environment (such as nutrition source and water column salinity) associated with seawater transgression into the lake are among the most important reasons for oil shales in the Songliao Basin being different from mudstone and oil shale in other rifted basins.展开更多
To determine geochemical indicators for depositional environment favored by terrestrial petroleum source rocks, we selected 40 source rock samples from the Late Cretaceous Qingshankou Formation (K2qn) and the first me...To determine geochemical indicators for depositional environment favored by terrestrial petroleum source rocks, we selected 40 source rock samples from the Late Cretaceous Qingshankou Formation (K2qn) and the first member of Nenjiang Formation (K2n1) in the Songliao Basin to qualify saturate fraction and aromatic fraction using GC-HRT (gas chromatography high reso lution time-of-flight mass spectrometry) and quantify important biomarkers using GC-MS. The results reveal that source rocks from the 1st member of Qingshankou Formation (K2qn1) are characterized by not only high contents of terpanes, regular ster anes and 4-methylsteranes but also high contents of dinosteranes, C31 steranes and aryl isoprenoids. Presence of specific bi omarkers like elementary sulfur and lanostanes indicates a depositional environment of lagoon characterized by water stratifi cation and high salinity. In the 2nd-3rd members of Qingshankou Formation (K2qn2+3), source rocks contain lower contents of biomarkers, indicating a depositional environment of shallow fresh-water lake delta. Source rocks in the K2n1 contain high contents of terpanes, regular steranes and 4-methylsteranes but lower contents of dinosteranes, C31 steranes and aryl isopre noids, indicating a depositional environment of fresh-brackish open lake characterized by low salinity and poor water stratifi cation, where organic matter is seriously altered by bacteria. Overall analysis shows that primary geochemical indicators for terrestrial petroleum source rocks are as follows: 1) C30 hopanes > 1500 ppm; 2) gammacerane >190 ppm; 3) C27 steranes >200 ppm; 4) 4-methylsteranes >100 ppm; 5) aryl isoprenoids > 3 ppm; 6) dehydroxyl-vitamin E >10 ppm.展开更多
基金Supported by the Central Guiding Local Science and Technology Development Special Project(ZY20B13)。
文摘By conducting experimental analyses, including thermal pyrolysis, micro-/nano-CT, argon-ion polishing field emission scanning electron microscopy (FE-SEM), confocal laser scanning microscopy (CLSM), and two-dimensional nuclear magnetic resonance (2D NMR), the Gulong shale oil in the Songliao Basin was investigated with respect to formation model, pore structure and accumulation mechanism. First, in the Gulong shale, there are a large number of pico-algae, nano-algae and dinoflagellates, which were formed in brackish water environment and constituted the hydrogen-rich oil source materials of shale. Second, most of the oil-generating materials of the Qingshankou Formation shale exist in the form of organo-clay complex. During organic matter thermal evolution, clay minerals had double effects of suppression and catalytic hydrogenation, which expanded shale oil window and increased light hydrocarbon yield. Third, the formation of storage space in the Gulong Shale was related to dissolution and hydrocarbon generation. With the diagenesis, micro-/nano-pores increased, pore diameter decreased and more bedding fractures appeared, which jointly gave rise to the unique reservoir with dual media (i.e. nano-scale pores and micro-scale bedding fractures) in the Gulong shale. Fourth, the micro-/nano-scale oil storage unit in the Gulong shale exhibits independent oil/gas occurrence phase, and shows that all-size pores contain oils, which occur in condensate state in micropores or in oil-gas two phase (or liquid) state in macropores/mesopores. The understanding about Gulong shale oil formation and accumulation mechanism has theoretical and practical significance for advancing continental shale oil exploration in China.
基金Supported by the the National Natural Science Foundation of China(U22A201550).
文摘On the basis of sorting out current understanding of solid bitumen (SB) in shales and taking organic-rich shales in the first member of the Cretaceous Qingshankou Formation in the Songliao Basin as an example, the definition, classification, occurrence and evolution path of SB are systemtically studied, and the indicative significance of SB reflectance (Rob) on maturity and its influence on the development of reservoir space are discussed and summarized. The results show that the difference of primary maceral types is primarily responsible for the different evolution paths of SB. Most of the pre-oil bitumen is in-situ SB with only a small amount being of migrated SB, while most of the post-oil bitumen and pyrobitumen are migrated SB. From the immature to early oil maturity stage, bituminite, vitrinite, and inertinite can be distinguished from SB based on their optical characteristics under reflected light, and alginite can be differentiated from SB by their fluorescence characteristics. Under scanning electron microscope, in-situ SB and migrated SB can be effectively identified. Rob increases linearly with increasing vitrinite reflectance (Ro), as a result of a decrease of aliphatic structure and the enhancement of aromatization of SB. Within the oil window three types of secondary pores may develop in SB, including modified mineral pores, devolatilization cracks and bubble holes. At a high maturity stage spongy pores may develop in pyrobitumen. Scanning electron microscopy combined with in-situ SEM-Raman spectroscopy can further reveal the structral information of different types of SB, thus providing crucial data for understanding for understanding OM migration paths, dynamics, and distances at micro-scale.
基金the National Natural Science Foundation of China (No. 40572079); the Program for New Century Excellent Talents in University (No. NCET-04-0345); the Venture Capital Foundation of PetroChina (No. 2005-01-02).
文摘In order to investigate the migration and accumulation efficiency of hydrocarbon natural gas in the Xujiaweizi fault depression, and to provide new evidence for the classification of its genesis, a source rock pyrolysis experiment in a closed system was designed and carried out. Based on this, kinetic models for describing gas generation from organic matter and carbon isotope fractionation during this process were established, calibrated and then extrapolated to geologic conditions by combining the thermal history data of the Xushen-1 Well. The results indicate that the coal measures in the Xujiaweizi fault depression are typical "high-efficiency gas sources", the natural gas generated from them has a high migration and accumulation efficiency, and consequently a large-scale natural gas accumulation occurred in the area. The highly/over matured coal measures in the Xujiaweizi fault depression generate coaliferous gas with a high δ^13C1 value (〉 -20‰) at the late stage, making the carbon isotope composition of organic alkane gases abnormally heavy. In addition, the mixing and dissipation through the caprock of natural gas can result in the negative carbon isotope sequence (δ^13C1 〉δ^13C2 〉δ^13C3 〉δ^13C4) of organic alkane gases, and the dissipation can also lead to the abnormally heavy carbon isotope composition of organic alkane gases. As for the discovery of inorganic nonhydrocarbon gas reservoirs, it can only serve as an accessorial evidence rather than a direct evidence that the hydrocarbon gas is inorganic. As a result, it needs stronger evidence to classify the hydrocarbon natural gas in the Xujiaweizi fault depression as inorganic gas.
基金Supported by the PetroChina Science and Technology Project(2012E-2603-06)
文摘Taking tight oil in Gaotaizi and Fuyu oil layers of the Upper Cretaceous Qingshankou Formation in northern Songliao Basin as an example, based on analyses of nuclear magnetic resonance and high pressure mercury injection, experiment methods of supercritical carbon dioxide displacement and extraction are firstly employed to quantify crude oil mobility in tight sand reservoirs with different lithologies and oil contents. The results show that, under the conditions of simulating the Cretaceous Qingshankou Formation in the northern Songliao Basin at a temperature of 76-89 °C and a pressure of 35-42 MPa, the lower limit of the porosity of the movable oil is4.4%, and the lower limit of the permeability is 0.015′10-3 mm2. The lower limit of the average pore throat radius is 21 nm. On this basis,a classification standard for three types of tight sand reservoirs is proposed. Type I reservoirs are characterized by the movable fluid saturation larger than 40%, the movable oil ratio(ratio of movable oil to total oil) greater than 30% and the starting pressure gradient in the range of 0.3-0.6 MPa/m; Type II reservoirs are characterized by the movable fluid saturation in the range of 10%–40%, the movable oil ratio in the range of 5%–30% and the starting pressure gradient in the range of 0.6–1.0 MPa/m; Type III reservoirs are characterized by the movable fluid saturation less than 10% in general, the movable oil ratio less than 5%, and the starting pressure gradient greater than1.0 MPa/m. The fluid mobility in tight sand reservoirs is mainly affected by diagenesis and sedimentary environment. Reservoirs with depth lower than 2000 m are dominated by type I reservoir, whereas those with greater depth are dominated by type I and II reservoirs.Reservoirs in inner delta-front facies are dominated by type I reservoir, whereas those in outer delta-front facies and shore-shallow lacustrine facies are dominated by type II and III reservoirs.
文摘1 Introduction The technology breakthrough in the exploration of shale gas and tight oil has greatly extended the global fossil fuel resources (Jia et al., 2012; Zou et al., 2012; Qiu et al., 2013). Although shale oil has been the global hot topic in the study of unconventional resources, there are varied definitions with respect to shale oil by different researchers.
基金Supported by China National Key Fundamental Research and Development Program (Grant No. 2006CB701404) and Petro China Oilfield Company Ltd.
文摘Several oil shale beds, over 10 m thick, occur at the base of the first member of the Upper Cretaceous Qingshankou Formation (K2qn1) in the Songliao Basin. They act both as excellent source rocks for conventional oil and as potential oil deposit for shale oil production. Here we combine micropaleon-tology with organic geochemistry to investigate the paleo-depositional environment and organic source characteristics of the oil shales and black shales. Our results indicate that algal remains are dominant microfossils in K2qn1 oil shales, and their relatively high abundance suggests a major algal thriving event during the oil shale deposition. The presence of fresh water and brackish water species, Sentusidinium, Vesperopsis and Nyktericysta, and marine or brackish water deltaic and lagoonal species such as Kiokansium and Dinogymniopsis demonstrate that this paleo-continental lake was influenced by marine transgressions at the time of K2qn1 oil shale formation. The extremely low pristine/phytane ratios, relatively high abundance of gammacerane and 4-methyl steranes, and low δ 13C values of C14-C37 n-alkanes in the oil shale organic extracts indicate the deposition of oil shales in anoxic and highly stratified water columns and the significant contribution of lacustrine algae to sedimentary organic matter. High molecular-weight paraffinic hydrocarbons with unusually high abundance of nC43, nC45, and nC47 may be related to special algal species associated with marine transgression events. The giant water body of Songliao paleo-lake and the change in the organic and chemical environment (such as nutrition source and water column salinity) associated with seawater transgression into the lake are among the most important reasons for oil shales in the Songliao Basin being different from mudstone and oil shale in other rifted basins.
基金supported by Major State Basic Research Development Program of China (Grant No. 2009CB219308) and Petro China Daqing Oilfield Company Ltd.
文摘To determine geochemical indicators for depositional environment favored by terrestrial petroleum source rocks, we selected 40 source rock samples from the Late Cretaceous Qingshankou Formation (K2qn) and the first member of Nenjiang Formation (K2n1) in the Songliao Basin to qualify saturate fraction and aromatic fraction using GC-HRT (gas chromatography high reso lution time-of-flight mass spectrometry) and quantify important biomarkers using GC-MS. The results reveal that source rocks from the 1st member of Qingshankou Formation (K2qn1) are characterized by not only high contents of terpanes, regular ster anes and 4-methylsteranes but also high contents of dinosteranes, C31 steranes and aryl isoprenoids. Presence of specific bi omarkers like elementary sulfur and lanostanes indicates a depositional environment of lagoon characterized by water stratifi cation and high salinity. In the 2nd-3rd members of Qingshankou Formation (K2qn2+3), source rocks contain lower contents of biomarkers, indicating a depositional environment of shallow fresh-water lake delta. Source rocks in the K2n1 contain high contents of terpanes, regular steranes and 4-methylsteranes but lower contents of dinosteranes, C31 steranes and aryl isopre noids, indicating a depositional environment of fresh-brackish open lake characterized by low salinity and poor water stratifi cation, where organic matter is seriously altered by bacteria. Overall analysis shows that primary geochemical indicators for terrestrial petroleum source rocks are as follows: 1) C30 hopanes > 1500 ppm; 2) gammacerane >190 ppm; 3) C27 steranes >200 ppm; 4) 4-methylsteranes >100 ppm; 5) aryl isoprenoids > 3 ppm; 6) dehydroxyl-vitamin E >10 ppm.